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WO2006001923A2 - Composite bistable nanoparticules-polymere utilise dans des dispositifs de memoire - Google Patents

Composite bistable nanoparticules-polymere utilise dans des dispositifs de memoire Download PDF

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Publication number
WO2006001923A2
WO2006001923A2 PCT/US2005/016741 US2005016741W WO2006001923A2 WO 2006001923 A2 WO2006001923 A2 WO 2006001923A2 US 2005016741 W US2005016741 W US 2005016741W WO 2006001923 A2 WO2006001923 A2 WO 2006001923A2
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WO
WIPO (PCT)
Prior art keywords
bistable
nanoparticles
electrically
electronic devices
bistable body
Prior art date
Application number
PCT/US2005/016741
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English (en)
Other versions
WO2006001923A3 (fr
Inventor
Yang Yang
Jianyong Ouyang
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The Regents Of The University Of California
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Filing date
Publication date
Application filed by The Regents Of The University Of California filed Critical The Regents Of The University Of California
Priority to US11/596,585 priority Critical patent/US7750341B2/en
Publication of WO2006001923A2 publication Critical patent/WO2006001923A2/fr
Publication of WO2006001923A3 publication Critical patent/WO2006001923A3/fr

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
    • H01B1/20—Conductive material dispersed in non-conductive organic material
    • H01B1/22—Conductive material dispersed in non-conductive organic material the conductive material comprising metals or alloys
    • G—PHYSICS
    • G11—INFORMATION STORAGE
    • G11C—STATIC STORES
    • G11C11/00—Digital stores characterised by the use of particular electric or magnetic storage elements; Storage elements therefor
    • G11C11/21—Digital stores characterised by the use of particular electric or magnetic storage elements; Storage elements therefor using electric elements
    • G11C11/22—Digital stores characterised by the use of particular electric or magnetic storage elements; Storage elements therefor using electric elements using ferroelectric elements
    • G—PHYSICS
    • G11—INFORMATION STORAGE
    • G11C—STATIC STORES
    • G11C13/00—Digital stores characterised by the use of storage elements not covered by groups G11C11/00, G11C23/00, or G11C25/00
    • G11C13/0002—Digital stores characterised by the use of storage elements not covered by groups G11C11/00, G11C23/00, or G11C25/00 using resistive RAM [RRAM] elements
    • G11C13/0009—RRAM elements whose operation depends upon chemical change
    • G11C13/0014—RRAM elements whose operation depends upon chemical change comprising cells based on organic memory material
    • G—PHYSICS
    • G11—INFORMATION STORAGE
    • G11C—STATIC STORES
    • G11C13/00—Digital stores characterised by the use of storage elements not covered by groups G11C11/00, G11C23/00, or G11C25/00
    • G11C13/0002—Digital stores characterised by the use of storage elements not covered by groups G11C11/00, G11C23/00, or G11C25/00 using resistive RAM [RRAM] elements
    • G11C13/0009—RRAM elements whose operation depends upon chemical change
    • G11C13/0014—RRAM elements whose operation depends upon chemical change comprising cells based on organic memory material
    • G11C13/0016—RRAM elements whose operation depends upon chemical change comprising cells based on organic memory material comprising polymers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y10/00—Nanotechnology for information processing, storage or transmission, e.g. quantum computing or single electron logic
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K10/00—Organic devices specially adapted for rectifying, amplifying, oscillating or switching; Organic capacitors or resistors having potential barriers
    • H10K10/20—Organic diodes
    • H10K10/23—Schottky diodes
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K10/00—Organic devices specially adapted for rectifying, amplifying, oscillating or switching; Organic capacitors or resistors having potential barriers
    • H10K10/50—Bistable switching devices
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K19/00—Integrated devices, or assemblies of multiple devices, comprising at least one organic element specially adapted for rectifying, amplifying, oscillating or switching, covered by group H10K10/00
    • H10K19/202—Integrated devices comprising a common active layer
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S977/00—Nanotechnology
    • Y10S977/70—Nanostructure
    • Y10S977/773—Nanoparticle, i.e. structure having three dimensions of 100 nm or less
    • Y10S977/774—Exhibiting three-dimensional carrier confinement, e.g. quantum dots
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S977/00—Nanotechnology
    • Y10S977/70—Nanostructure
    • Y10S977/778—Nanostructure within specified host or matrix material, e.g. nanocomposite films
    • Y10S977/779—Possessing nanosized particles, powders, flakes, or clusters other than simple atomic impurity doping
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S977/00—Nanotechnology
    • Y10S977/70—Nanostructure
    • Y10S977/778—Nanostructure within specified host or matrix material, e.g. nanocomposite films
    • Y10S977/783—Organic host/matrix, e.g. lipid
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S977/00—Nanotechnology
    • Y10S977/70—Nanostructure
    • Y10S977/81—Of specified metal or metal alloy composition
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S977/00—Nanotechnology
    • Y10S977/902—Specified use of nanostructure
    • Y10S977/932—Specified use of nanostructure for electronic or optoelectronic application
    • Y10S977/943—Information storage or retrieval using nanostructure
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/26—Web or sheet containing structurally defined element or component, the element or component having a specified physical dimension
    • Y10T428/268—Monolayer with structurally defined element
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/26—Web or sheet containing structurally defined element or component, the element or component having a specified physical dimension
    • Y10T428/269—Web or sheet containing structurally defined element or component, the element or component having a specified physical dimension including synthetic resin or polymer layer or component

Definitions

  • the present invention relates generally to electrically bistable materials that can be converted from a low conductance (electrically off) state to a high conductance (electrically on) state by application of an electrical field to the material. More particularly, the present invention is directed to bistable materials that are composed of a polymer matrix in which nanoparticles are dispersed to provide the polymer with the desired bistable properties.
  • Nanometer materials exhibit peculiar electrical, optical and magnetic properties that are different from bulk materials and atoms [1-4].
  • the electronic materials in nanometer size are especially interesting due to the quantum effect of the electron. New phenomena have been observed on the nanometer materials, such as "Coulombic blockage", surface-enhanced Raman signal, and size-determined energy gap. Charge transfer related the metal nanoparticle has gained much attention [5-8]. It was observed that metal nanoparticles can be charged positively or negatively.
  • the device with a polymer film containing 2-naphthalene-capped Au nanoparticles sandwiched between two aluminum (Al) electrodes exhibits an electrical transition to a high conductivity state under a high electric field.
  • This device can be used as write-once-read- many electronic memory [H].
  • a polymer matrix that contains the appropriate amount of capped nanoparticles provides a bistable body that can be used in a wide variety of bistable devices.
  • the capped nanoparticles, which are dispersed in the polymer matrix include metal nanoparticles that are coated with aromatic thiol molecules.
  • the present invention covers electrically bistable bodies that are intended for use in electronic devices wherein the bistable body is converted from a low conductance state to a high conductance state by application of an appropriate electrical potential.
  • the bistable body is composed of a polymer matrix in which a sufficient amount of capped nanoparticles are dispersed to provide a material which is electrically convertible from the low conductance state to the high conductance state.
  • the capped nanoparticles are composed of metal nanoparticles that have a surface on which is located a coating of aromatic thiol molecules.
  • the present invention not only covers the bistable body, but also any of the many bistable devices in which the bistable body is used, such as memory devices.
  • the invention is based on the discovery that an electric-field induced electrical transition was observed on a device with a polystyrene film containing 2- naphthalenethiol-capped Au nanoparticles sandwiched between two Al electrodes. Before the electrical transition the device exhibited a very low current controlled by the charge injection from the Al electrode into the polymer film.
  • FIG. 1 is a diagrammatic representation of an exemplary bistable device, which includes a bistable body in accordance with the present invention.
  • FIG. 2 is an I-V curve of Al/PS+Au-NT/Al. The arrows indicate the bias- scanning directions and the structure under test is shown in the insert.
  • FIG. 3 a graph of Iogl-V 1/2 (a) and Logl-logV (b) of the device Al/PS+Au- NT/A1 before (a) and after (b) the electrical transition.
  • FIG. 4 is an asymmetrical IV curve for Al/PS+Au-NT/Al after the electrical transition.
  • FIG. 14 FIG.
  • FIG. 5(a) is a schematic representation of charge transfer from 2- naphthalenethiol to Au nanoparticle under electric field E. The arrow indicates the direction of the electric field E.
  • FIG. 5(b) is a schematic representation of the energy band structure and charge injection from Al into 2-naphthalenethiol before (left) and after (right) electrical transition. The dots on the HOMO represent the electrons.
  • FIG. 6 is a graph of the IV curve of and exemplary device Al/Au-BET+PS/Al. The inset is the chemical structure of 2-benzeneethanethiol (BET).
  • FIG. 7 a graph showing the results of a stress test of an exemplary device in the charge-transport-dominant state at a voltage of IV. DETAILED DESCRIPTION OF THE INVENTION
  • a bistable electrical device in accordance with the present invention is shown generally at 10 in FIG. 1.
  • the device 10 includes a bistable body 12 which is sandwiched between a first electrode 14 and a second electrode 16.
  • the bistable body 12 is shown in the form of a layer. However, it will be understood that the bistable body can be provided in any number of different shapes. Bistable bodies in the form of a thin layer or film are preferred since fabrication techniques for forming thin films are well known.
  • the bistable body 12 includes a first surface 18 which defines a first electrode location on which the first electrode 14 is attached.
  • a second surface 20 is located on the other side of the bistable body 12. This second surface 20 defines a second electrode location on which the second electrode 16 is attached.
  • the bistable electrical device 10 is connected to an electronic control unit 22 via electrical connections 24 and 26.
  • the control unit 22 is capable of providing an electrical voltage bias across the bistable body 12 via the two electrodes 14 and 16 to convert the bistable body between low resistance and high resistance states.
  • the control unit is capable of, among other things, measuring current to determine the electrical resistance of the bistable body.
  • Aluminum (Al) is the preferred electrode material.
  • the electrode can be made from other metals or conductive oxides (like indium tin oxide) that are known for use as electrode materials.
  • the nanoparticles which are capped with the aromatic thiol molecules to form the "capped nanopartilces" may be made from metal and metal alloys of Au, Pt, Ag and the like.
  • the particles have sizes that are preferably on the order of 10 nm or less. Larger particles may be used if desired. However, as the particle size increases, it becomes more difficult to dissolve the particles in organic solvents.
  • Polystyrene films are preferred as the polymer matrix. However, other polymers may be used including poly(methylmethacrylate), poly(vinyl pyridine) and the like.
  • the preferred concentration of capped nanoparticles in the polymer matrix ranges from 0.05 to 1.2% by weight in solution, which is equivalent to 4 to 50 weight percent in the resulting polymer film. Concentrations of capped nanoparticles outside this range may be used, if desired provided that the desired transition is still achieved.
  • the thickness of the film (polymer matrix) will typically range from 20 to 100 nm.
  • 2-naphthalenethiol is the preferred molecule for capping the nanoparticles.
  • other aromatic thiol molecules may be used in place of 2-naphthalenethiol.
  • 2-benzeneethanethiol may be used in place of 2-naphthalenethiol, but it does not work quite as well.
  • the capping molecules can be any molecules with a thiol group (or disulfide and others, which can form a S-Au bond on Au and other metal nanoparticles) and a conjugated ring moiety.
  • the nanoparticles are coated with the aromatic thiol molecules according to known procedures (9,10) to form the capped nanoparticles.
  • 0.62 g HAuCl 4 3H 2 O was dissolved in 50 ml water and mixed with 160 ml p-xylene solution of 3 g tetraoctylammonium bromide.
  • the organic phase was isolated and 0.28g 2- naphthalenethiol was added.
  • the formation of the Au nanoparticles was completed by adding 50 ml aqueous solution of 0.76 g NaBH 4 dropwisely into the organic solution under vigorous stirring.
  • the Au nanoparticles were purified by washing with 300 ml methanol for at least three times.
  • the entire surface of the nanoparticle be substantially covered with a monolayer of aromatic thiol molecules.
  • the surface does not have to be completely covered, so long as the desired bistable effect is still obtained.
  • the exact amount of surface coverage required to obtain capped nanoparticles that may be used in accordance with the present invention can be determined by routine experimentation. Conversely, the upper limit of coating thickness may also be determined by routine experimentation.
  • 2-naphthalenethiol capped Au nanoparticles (Au- 2NT NPs) were prepared by the two-phase arrested method [10]. The surface of the nanoparticle was substantially covered with a monolayer of 2-naphthalenethiol molecules.
  • the device which has a device structure as shown in FIG. 1, was fabricated using the following process.
  • the bottom Al electrodes were deposited on the glass substrates by the thermal evaporation in vacuum of about IxIO 5 Torr.
  • the active film was formed by spin-coating 1,2-dichlorobenzenic solution of 1.2% by weight polystyrene and 0.4% by weight Au-2NT NPs. This film has a thickness of about 50 nm.
  • the top Al electrodes were deposited perpendicular to the bottom electrodes.
  • the top and bottom Al electrodes have a line width of 0.2 mm. Al/Au-2NT NPs+PS/Al is used to represent this device.
  • I- V curves were tested using HP 4155 semiconductor analyzer in vacuum or in air.
  • the geometry of 2-naphthalenethiol was optimized with semi-empirical AMI and HOMO-LUMO energies were calculated with DFT B3LYP/6- 31 G + (d, p).
  • the IV curve of this device is shown in FIG. 2.
  • the device exhibited a very low current in the low voltage range at the first scan.
  • the current is in the range of 0.1 nanoampere (nA) at 2V.
  • An electrical transition occurred under a high electric field. A rapid increase of the current took place at voltage higher than 7 volt. Hysteria of current was observed during the subsequent scan and the current at the second scan is much higher than at the first scan.
  • the current at 2V at the second scan is higher than at the first scan by more than three orders in magnitude.
  • the current was symmetrical in the two-biased direction in the voltage less than 3V for the device in the CI state. It turned into asymmetrical in the CT state.
  • the biased direction which leads to the electrical transition, is defined as the positive bias direction
  • the current along the negative biased direction is higher than during the positive bias scan.
  • FIG. 4 The current at -3 V reaches almost ten times as that at 3V.
  • This asymmetrical IV curve for the device in the CT state suggests that the electric field may induce polarization on Au-2NT NPs.
  • 5b is the energy diagram of the work function (4.1 eV) of the Al electrode and the highest occupied molecular orbital (HOMO) (HOMO) (5.8 eV) and the lowest unoccupied molecular orbital (LUMO) (1.4 eV) levels of 2NT.
  • HOMO highest occupied molecular orbital
  • LUMO lowest unoccupied molecular orbital
  • FIG. 7 depicts the results of a stress test of the device at IV after the electronic transition. At the beginning, the current decreases but then becomes stable. This initial experiment indicates that the device could be stable in this high conductivity state for more than 60 hours in air. This stability should be greatly improved when the conditions are optimized.
  • the electronic transition and the stability of the device in the CT state suggest that this device could be used as write-once-read-many electronic memory.
  • electric-field induced transition was observed on the device Al/Au-2NT+PS/Al.
  • FIG. 5(a) is a diagrammatic representation showing an Au nanoparticle capped with four 2-naphthalenethiols. Actually, as mentioned above, the whole surface of the Au nanoparticle is coated with a monolayer of 2-naphthalenthiols.

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  • Engineering & Computer Science (AREA)
  • Computer Hardware Design (AREA)
  • Physics & Mathematics (AREA)
  • Chemical & Material Sciences (AREA)
  • Dispersion Chemistry (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • Semiconductor Memories (AREA)
  • Polymers With Sulfur, Phosphorus Or Metals In The Main Chain (AREA)
  • Polyoxymethylene Polymers And Polymers With Carbon-To-Carbon Bonds (AREA)
  • Compositions Of Macromolecular Compounds (AREA)

Abstract

La présente invention concerne un corps électriquement bistable utilisé dans des dispositifs électroniques. Ce corps bistable passe d'un état de faible conductivité à un état de haute conductivité et comprend une matrice polymère dans laquelle une quantité suffisante de nanoparticules recouvertes sont dispersées de manière à faire passer le corps bistable d'un état de faible conductivité à un état de haute conductivité lors de l'application d'un champ électrique. Les nanoparticules recouvertes sont des nanoparticules métalliques qui ont été recouvertes d'un thiol aromatique.
PCT/US2005/016741 2004-05-17 2005-05-12 Composite bistable nanoparticules-polymere utilise dans des dispositifs de memoire WO2006001923A2 (fr)

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Application Number Priority Date Filing Date Title
US11/596,585 US7750341B2 (en) 2004-05-17 2005-05-12 Bistable nanoparticle-polymer composite for use in memory devices

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US57214504P 2004-05-17 2004-05-17
US60/572,145 2004-05-17

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WO2006001923A2 true WO2006001923A2 (fr) 2006-01-05
WO2006001923A3 WO2006001923A3 (fr) 2007-11-22

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EP1997814A1 (fr) * 2007-05-28 2008-12-03 Samsung Electronics Co., Ltd. Nanoparticule métallique fonctionnalisée, couche tampon l'incorporant et dispositif électronique incluant la couche tampon
JP2010508123A (ja) * 2006-10-31 2010-03-18 アボット ダイアベティス ケア インコーポレイテッド 注入装置および方法
KR101258284B1 (ko) * 2006-05-22 2013-04-25 삼성전자주식회사 메모리 소자 구동 회로

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KR101223718B1 (ko) * 2005-06-18 2013-01-18 삼성디스플레이 주식회사 나노 도전성 막의 패터닝 방법
JP2010161312A (ja) * 2009-01-09 2010-07-22 Sharp Corp 有機薄膜トランジスタおよびその製造方法
WO2012054715A2 (fr) * 2010-10-22 2012-04-26 Drexel University Procédés de fabrication de points quantiques hydrosolubles
US10253187B2 (en) * 2011-11-08 2019-04-09 Samsung Electronics Co., Ltd. Nano-structure of block copolymer and method of manufacturing the same

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